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• W4385291339 endingPage "10526" @default.
• W4385291339 startingPage "10511" @default.
• W4385291339 abstract "Molybdenum sulfide-based catalysts are widely used for hydrotreatment, hydrogen evolution, and many other reactions. Recently, we demonstrated that not only the edges of MoS2 slabs but few-atom ultradispersed MoSx clusters also possess high intrinsic activity. However, the structure and genesis of such ultradispersed species remain unknown. Herein, we present a comparative study of MoSx catalysts ultradispersed on different supports (carbons, SiO2, Al2O3, and TiO2). Evolution of the Mo species during sulfidation and hydrodesulfurization (HDS) reaction was studied by means of operando quick X-ray absorption spectroscopy at the Mo K-edge, assisted by chemometric analysis (multivariate curve resolution with alternating least squares). Significant differences of the structure of Mo species and their temperature evolution as a function of support were observed. The sulfidation pathway involves the formation of oxysulfide and sulfur-rich MoS3-like intermediates, which are further transformed into the final MoSx clusters. As compared with MoS2 nanoslabs, the coordination numbers of Mo in the ultradispersed clusters are decreased, and the interatomic Mo–S and Mo–Mo distances are shortened. Other characterizations, in particular, STEM-ADF, confirm that few-atom clusters and single-atom species are predominant in all the catalysts. The materials show high activity per Mo atom in the HDS of thiophene, varying in steps with MoSx dispersion, as determined from XAS, in the sequence: Mo/carbons > Mo/TiO2 > Mo/Al2O3 ≈ Mo/SiO2." @default.
• W4385291339 created "2023-07-27" @default.
• W4385291339 creator A5016452415 @default.
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• W4385291339 creator A5016945436 @default.
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• W4385291339 creator A5040224847 @default.
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• W4385291339 creator A5043595079 @default.
• W4385291339 date "2023-07-27" @default.
• W4385291339 modified "2023-10-18" @default.
• W4385291339 title "Genesis of Active Phase and Support Effect in Ultradispersed Mo Sulfide Catalysts" @default.
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